CHEMICAL ENGINEERING JOURNAL
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2024
·
IF 13.3
Fengshun Wu,Li Zeng,Lihua Zhu,Weizhen Wang,Chenghao Cao,Zhiqing Yang,Congxiao Shang,Hengqiang Ye,Zhengxiao Guo
Methanol and ethanol are liquid carriers of hydrogen, convenient and safe to store and transport, particularly of interest as mobile and marine fuels. These can be directly fed into a fuel cell to impart clean energy efficiently, only if their conversion can be cost-effectively catalyzed. In this regard, a cooperative catalyst is developed with atomic Pd species, in the form of single atoms and nanoclusters, dispersed over non-noble bi-metallic CoNi alloy nanoparticles, further supported on reduced graphene oxide (rG) (Pd@CoNi/rG). The catalyst demonstrates a methanol (ethanol) oxidation, MOR (EOR), mass activity (MA) of 1.730 (3.917) A mg −1 Pd (or Pt) , 4.55 (60.26) times greater than that of the commercial 20 wt% Pt/C and 8.65 (20.61) times higher than that of the commercial 20 wt% Pd/C, respectively. More importantly, the catalyst shows excellent stability, maintaining 83.7% (93.7%) of the initial performance after chronoamperometry (CA) for 50000 s in a solution of 1 M KOH + 1 M CH 3 OH (CH 3 CH 2 OH). It significantly out-performs other mono-/bi- metallic counterparts, e.g., Co/rG, Ni/rG, Pd/rG, CoNi/rG, Pd@Co/rG and Pd@Ni/rG, due to its unique cooperative nanostructure with synergistic effects of the different metal (Pd, Co and Ni)-related species.
研究领域:
材料科学
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电化学
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能源科学
✓ 已验证
产品关联
DOI
高影响因子
BIORESOURCE TECHNOLOGY
·
2014
·
IF 5.039
Riyang Shu,Jinxing Long,Zhengqiu Yuan,Qi Zhang,Tiejun Wang,Chenguang Wang,Longlong Ma
An efficient lignin depolymerization process with highly controllable product distribution was presented using metal chloride (MCl x ) cooperated with Pd/C. The catalytic performances of MCl x were investigated. The effect of reaction conditions on the lignin depolymerization and products distribution were also studied. Results showed that more than 35.4% yield of phenolic monomer including 7.8% phenols and 1.1% guaiacols could be obtained under optimized condition. And the product distribution can be efficiently controlled by the modification of the metal cation through different pathway of Lewis acid catalysis and coordination catalysis. Furthermore, the Pd/C catalyst showed an excellent recyclability, where no significant loss of the catalytic activity was exhibited after 3 runs. Moreover, the product control mechanism was proposed.
研究领域:
化学工程
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催化科学
✓ 已验证
产品关联
DOI
PubMed
高影响因子
Journal of CO2 Utilization
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2016
·
IF 4.764
Xiying Fu,Dagang Zhou,Kai Wang,Huanwang Jing
Pd/C was found to be an excellent catalyst in the coupling reaction of carbon dioxide and epoxides with tetrabutylammonium iodide (TBAI) as cocatalyst and the corresponding cyclic carbonates were obtained in good yields and high selectivities. 3-Chloropropylene carbonate was synthesized under extremely mild conditions of room temperature and atmosphere. The proposed mechanism was also calculated and confirmed by DFT. The palladium catalyst could be simply recycled and reused for 5 times without significant loss of activity.
研究领域:
化学
·
环境科学
✓ 已验证
产品关联
DOI
高影响因子
CHEMICAL ENGINEERING JOURNAL
·
2023
·
IF 15.1
Cong Wu,Qinglong Liu,Yu Zhan,Wei Tan,Xiaoqian Wei,Qing Tong,Haiqin Wan,Lin Dong
Indoor volatile organic compounds (VOCs), represented by toluene, can pose a serious threat to human health. In this work, a series of Pd/TiO 2 catalysts with different surface structures ( i.e. , dispersion/valence of Pd species, surface Ti 3+ /oxygen defect concentration and Pd-TiO 2 interactions, etc. ) was constructed by various methods. It was found that the Pd/TiO 2 catalyst prepared by one-step reduction of NaBH 4 method (Pd/TiO 2 -N) with metallic Pd particles possessed more surface Ti 3+ /oxygen defects and stronger Pd-TiO 2 interaction than Pd/TiO 2 catalysts prepared by ethylene glycol reduction loading method (Pd/TiO 2 -E) and incipient wetness impregnation method (Pd/TiO 2 -I). Further photochemical characterizations and reaction mechanism study revealed that the relatively higher concentration of Pd 0 species on Pd particles, stronger Pd-TiO 2 interaction, and more surface Ti 3+ /oxygen defects on Pd/TiO 2 -N could facilitate the generation of more reactive oxygen species (ROS) under light irradiation. The partial oxidation of toluene to benzyl alcohol/benzaldehyde/benzoic acid and the subsequent ring-opening process were found to be highly determined by the valence states of Pd particles and the concentration of surface Ti 3+ /oxygen defects. This work provides instructive insights into the construction of highly efficient Pd/TiO 2 catalysts for the removal of indoor VOCs.
研究领域:
环境科学
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材料科学
✓ 已验证
产品关联
DOI
高影响因子
MICROPOROUS AND MESOPOROUS MATERIALS
·
2017
·
IF 3.615
Hong Jiang,Songlin Xue,Yefei Liu,Weihong Xing,Rizhi Chen
The Pd@ZIF-L catalysts with uniform crosshair-star shape and a size of about 20 μm were synthesized by an assembly method, in which a two-dimensional layered zeolitic imidazolate framework-L (ZIF-L) was used as the support to immobilize Pd nanoparticles . Their catalytic activities were evaluated by the catalytic reduction of p -nitrophenol to p -aminophenol. The results highlight that the physical-chemical and catalytic properties of the Pd@ZIF-L catalysts are greatly affected by the synthesis temperature. The temperature variation can make the catalysts transform from two-dimensional flakes to zero-dimensional spheres. High temperature is beneficial for increasing Pd loading and encapsulating Pd nanoparticles within the ZIF-L matrix. However, under the temperature larger than 30 °C, the dense dia(Zn) structures are formed. Increasing Pd loading in the Pd@ZIF-L catalysts leads to a significantly higher p -nitrophenol conversion. The relative dense structure of the as-synthesized catalysts makes p -nitrophenol access the active centers difficultly and a lower catalytic activity is observed. These findings would aid the development of high-performance Pd@ZIF-L catalysts.
研究领域:
材料科学
·
催化化学
✓ 已验证
DOI
高影响因子
SEPARATION AND PURIFICATION TECHNOLOGY
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2024
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IF 8.1
Meiling Chen,Xingyu Liu,Xiaole Weng,Renna Li,Zhongbiao Wu
The control of low-concentration methane (CH 4 ) emissions is a critical component of the ‘dual carbon’ strategy, and catalytic combustion technology focused on catalyst design is recognized as a promising avenue for achieving it. However, the zeolite-based catalysts are highly prone to deactivation under hydrothermal environments, thus limiting their practical applicability. Herein, we have utilized layered double hydroxides (LDHs) as precursors and integrated them with Pd/M through a co-precipitation method to fabricate Pd/M@CoAlO composite catalysts with a core–shell structure, focused on the impact of CoAlO morphology on the activity and stability for CH 4 oxidation. It revealed that the incorporation of CoAlO significantly enhanced the catalytic combustion efficiency and the hydrothermal stability of Pd/M. Furthermore, an increase in the calcination temperature led to a progressive degradation of the sheet-like or petal-shaped structure of CoAlO within the Pd/M@CoAlO composite catalysts. This structural collapse eventually resulted in the formation of CoAlO dense particles that enveloped the Pd/M, adversely affecting the adsorption of oxygen and the exposure of active sites. This work underscores the importance of morphological control, providing significant guidance for the strategic design and development of catalysts tailored for CH 4 catalytic combustion.
研究领域:
环境科学
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催化材料学
✓ 已验证
产品关联
DOI
高影响因子
Journal of Materials Chemistry A
·
2017
·Vol. 5
·期 6
·2619-2628
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IF 8.867
Yuzhen Zhu,Zaixiang Xu,Wenya Jiang,Shuxian Zhong,Leihong Zhao,Song Bai
The utilization of a metal cocatalyst is a promising route to improve the solar-to-chemical conversion efficiency of semiconductor-based photocatalysts. The efficiency of the improvement is greatly dependent on the architectural structure of the metal cocatalysts, especially the catalytically active sites on the surface of the cocatalysts. In this article, Pd nanosheets with different sizes have been hybridized with TiO2 nanosheets to disclose how the edge of Pd cocatalysts influences the photocatalytic performance of TiO2–Pd hybrid structures in the reduction of CO2 to fuels. It was found that the highest photocatalytic activity was realized by small Pd nanosheets with the highest edge density on the TiO2 nanosheets. The reason is that the edges of the nanosheets act as the highly active sites for the CO2 reduction reaction. To further verify the edge-dependent photocatalytic performance, Pd nanorings were also deposited on the TiO2 nanosheets, which further improve the photocatalytic activity as compared with original nanosheets resulting from the additional edge sites exposed on the side of the hollow interior in the rings. This work underlines the importance in the edge engineering on the surface of cocatalysts in realizing high-performance photocatalytic applications.
研究领域:
材料科学
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能源化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
CATALYSIS COMMUNICATIONS
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2014
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IF 3.32
Xuanduong Le,Zhengping Dong,Zhicheng Jin,Qingqing Wang,Jiantai Ma
In this study, a novel Pd(II) complex functionalized core–shell magnetic mesoporous catalyst (Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II)) was synthesized by a simple cost effective procedure. It was characterized by transmission electron microscopy, X-ray diffraction, Fourier transform infrared spectroscopy, X-ray photoelectron spectroscopy, vibrating sample magnetometer, and nitrogen physical adsorption. The Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II) catalyst offered high surface area and exhibited excellent activity towards Suzuki–Miyaura cross-coupling reaction of halides with aryl boronic acids in ethanol in air. The Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II) catalyst was stable, reusable, and conveniently recovered by applying an external magnetic field. Moreover, it provided 91% conversion after the sixth catalytic run. The Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II) catalyst examined in this study combined both the efficiency of a homogeneous catalyst and the durability of a heterogeneous catalyst. The results revealed that the Fe 3 O 4 @SiO 2 @mSiO 2 –Pd(II) catalyst is promising as a candidate for various Pd-based catalytic applications.
研究领域:
化学
·
材料科学
✓ 已验证
产品关联
DOI
高影响因子
Catalysis Science & Technology
·
2015
·Vol. 5
·期 6
·3333-3339
·
IF 5.426
Dong-Mei Lv,Zhong-Ning Xu,Si-Yan Peng,Zhi-Qiao Wang,Qing-Song Chen,Yumin Chen,Guo-Cong Guo
(Pd–CuCl2)/γ-Al2O3 catalyst with excellent activity and selectivity has been successfully developed for vapor-phase carbonylation of methyl nitrite to dimethyl carbonate (DMC). It has been demonstrated that Cl− is necessary for the superior selectivity (99.8%) to DMC, and that Cl− and Cu2+ have a synergetic effect. The Lewis acid sites of the γ-Al2O3 support may be suitable for vapor-phase carbonylation of methyl nitrite to DMC. Moreover, the catalytic mechanism of DMC formation on the (Pd–CuCl2)/γ-Al2O3 catalyst has been reasonably proposed based on the results of XPS and in situ diffuse reflectance infrared spectroscopy. The intermediate Cl–Pd(II)–COOCH3 is the key factor for the synthesis of DMC.
研究领域:
催化
·
化学工程
·
无机化学
✓ 已验证
产品关联
DOI
高影响因子
GREEN CHEMISTRY
·
2020
·Vol. 22
·期 13
·4341-4349
·
IF 9.48
Yuxue Xiao,Qingwei Meng,Xiaoli Pan,Chao Zhang,Zaihui Fu,Changzhi Li
para-Xylene (PX) is a basic building block of polyethylene terephthalate, which is currently produced from petroleum resources. Developing a renewable route to PX is highly desirable to address both economic and environmental concerns. Several attempts used noble metal catalysts, e.g. Pd/Al2O3, to synthesize PX from biomass-derived 4-methyl-3-cyclohexene-1-carboxaldehyde (4-MCHCA), but suffered from a severe decarbonylation reaction, resulting in toluene as the main product. In this paper, we report an FeOx modification strategy to suppress the decarbonylation reaction on a Pd/Al2O3 catalyst, leading to a drastic shift in selectivity towards PX with a yield up to 81% via a cascade dehydroaromatization–hydrodeoxygenation (DHA–HDO) pathway. Characterization and control experiments revealed that the electron density of Pd sites decreased in an FeOx-modified Pd/Al2O3 catalyst compared to Pd/Al2O3, thus tuning the preferential adsorption mode of the substrate from η2-(C,O), the key transition state of the decarbonylation reaction, to the η1-(O) mode that favors the hydrodeoxygenation process. Notably, this designed catalyst is highly stable and is readily applicable in the selective synthesis of a broad range of desired aromatic chemicals via the same DHA–HDO pathway from cyclohex-3-enecarbaldehyde derivatives. Overall, this work develops a controllable catalyst modification strategy that tailors an efficient catalyst for petroleum-independent bio-PX synthesis.
研究领域:
催化化学
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可再生资源化学
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环境科学
✓ 已验证
产品关联
DOI
高影响因子
Molecular Catalysis
·
2021
·
IF 5.062
Jing Zhao,Hucheng Zhang,Haiyan Wang,Jianji Wang
A highly attractive aim is to turn CO 2 into useful chemicals selectively and efficiently, but it still retains great challenging to understand the relations between catalytic performances and interface properties. Here, we report an alternative solution to relate the catalytic activity with the strengths of Lewis acids and bases on the Pd-CoO x interfaces. CoO∙TiO 2 /TiO 2 and CoO x /TiO 2 possess the wide spectrum of Lewis acid/base centres, and give the low selectivity and conversion. The introduction of Pd can focus them on the intrinsic centres, and makes Pd-CoO∙TiO 2 /TiO 2 and Pd-CoO x /TiO 2 represent the ideal catalysis. With temperature-programmed desorptions of CO 2 , CO and NH 3 , it is evidenced that the catalytic hydrogenations of CO 2 to CO, CH 4 and CH 3 OH depend on the cooperation of the Lewis acidic/alkaline centres on the interfaces. The studies provide guidelines for rational design and synthesis of heterogeneous catalysts including but not limited to CO 2 hydrogenation.
研究领域:
化学工程
·
催化科学
✓ 已验证
产品关联
DOI
高影响因子
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
·
2024
·
IF 8.1
Ruiting Li,Tengyang Gao,Yao Wang,Yan Chen,Wen Luo,Yang Wu,Yu Xie,Yong Wang,Yifan Zhang
The application of metal catalysis has gained prominence as a study area in recent years. In this work, we use adsorptive reduction and calcination to create Au–Pd alloy catalysts on COCN-2 with varying metal loadings. The plasma resonance effect of the alloys increases the photoresponse of the catalysts, and the engineering of nitrogen defects strengthens the strong bonds between Au–Pd alloy particles and carbon nitride graphite, optimizing the electronic structure, encouraging electron-directed migration, and increasing the efficiency of the reduction reaction. As a result, the efficiency of hydrogen generation by the Au–Pd 0.6 /COCN-2 catalyst is 5.089 mmol g −1 h −1 , which is 2367 times higher than that of the g-C 3 N 4 catalyst. Our findings highlight the crucial part that flaws play in strengthening the strong bonds that exist between the metal and the support, which enhances photocatalytic hydrogen generation. This work offers insightful information about creating effective photocatalysts.
研究领域:
材料科学
·
催化化学
✓ 已验证
产品关联
DOI
高影响因子
危险品化学品经营许可证（带存储）